Definitely upgrade the GPU first. More often than not, a faster cpu will improve the framerate a bit, but a faster gpu will improve the framerate a lot. I've also got a 955 which i've had running at 3.75GHz for the last 4 years and i'm still not feeling the need to upgrade it but i'm feeling the need to upgrade my 6970 already. (which by all accounts is pretty much identical in performance to your 570) The only games i find running slow on my system are graphically heavy like crysis 2/3, which need to be run at very high as ultra/extreme is too much for the gpu. (like tressFX on tomb raider or ultra ambient occlusion on bioshock ultimate)
Overclocking the CPU NB is a wise move. Mine is running at 2662MHz. IIRC the voltage is at 1.25V for the CPU NB and 1.45V for the cpu. (older C2 stepping, needs plenty of juice) I have had it up at 2.9GHz with 1.425V and the cpu just over 4GHz with 1.55V but that just puts unnecessary strain on everything. If you increase the bus speed, (which isn't a bad idea) make sure to keep the HT-link speed very close to 2000mhz. (slightly under is fine as it doesn't affect performance. Over 2GHz can have a severe affect on stability.)
If it helps, I run the following settings:
FSB - 242
CPU x15.5 = 3751 @ 1.456V
CPU NB x11 = 2662 @ 1.250V
HT-link x8 = 1936
Memory x6.66 = 1612 @ 1.65V